ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH Göttingen, Germany 10.5194/acp-12-1229-2012 A simple relationship between cloud drop number concentration and precursor aerosol concentration for the regions of Earth's large marine stratocumulus decks Hegg D. A. 1 Covert D. S. 1 Jonsson H. H. 2 Woods R. K. 2 Department of Atmospheric Sciences, University of Washington, Seattle, WA, USA Meteorology Department, Naval Post Graduate School, Monterey, CA, USA 01 02 2012 12 3 1229 1238 This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited. This article is available from http://www.atmos-chem-phys.net/12/1229/2012/acp-12-1229-2012.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/12/1229/2012/acp-12-1229-2012.pdf

Aircraft–based measurements of cloud condensation nuclei (CCN), accumulation mode and Aitken mode number concentrations, cloud drop number concentration (CDNC), and selected ancillary measurements are presented for the three large, semi-permanent marine stratocumulus decks of the earth (in the Pacific offshore of California and Chile and in the Atlantic offshore of Namibia). Based on these data, a simple linear relationship between CDNC and the accumulation mode number concentration (AMNC) is derived via regression. The slope of the regression is 0.72 ± 0.04 with an <i>R</i><sup>2</sup> of 0.90, higher than those found for CDNC-CCN linear regressions. Explanations of the relatively favorable CDNC-AMNC relationship and its utility for climate studies are discussed.

 References Allen, G., Coe, H., Clarke, A., Bretherton, C., Wood, R., Abel, S. J., Barrett, P., Brown, P., George, R., Freitag, S., McNaughton, C., Howell, S., Shank, L., Kapustin, V., Brekhovskikh, V., Kleinman, L., Lee, Y.-N., Springston, S., Toniazzo, T., Krejci, R., Fochesatto, J., Shaw, G., Krecl, P., Brooks, B., McMeeking, G., Bower, K. N., Williams, P. I., Crosier, J., Crawford, I., Connolly, P., Allan, J. D., Covert, D., Bandy, A. R., Russell, L. M., Trembath, J., Bart, M., McQuaid, J. B., Wang, J., and Chand, D.: South East Pacific atmospheric composition and variability sampled along 20° S during VOCALS-REx, Atmos. Chem. Phys., 11, 5237–5262, http://dx.doi.org/10.5194/acp-11-5237-2011doi:10.5194/acp-11-5237-2011, 2011. Baumgardner, D., Strapp, W., and Dye, J. E.: Evaluation of the forward scattering aerosol spectrometer probe, Part II: Corrections for coincidence and dead-time losses, J. Atmos. Oceanic Technol., 2, 626–632, 1985. Bellouin, N., Jones, A., Haywood, J., and Christopher, S. A.: Updated estimate of aerosol direct radiative forcing from satellite observations and comparison against the Hadley Centre climate model, J. Geophys. Res., 113, D10205, http://dx.doi.org/10.1029/2007JD009385doi:10.1029/2007JD009385, 2008. Bi, X. H., Zhang, G. H., Li, L., Wang, X. M., Li, M., Sheng, G. Y., Fu, J. M., and Zhou, Z.: Mixing state of biomass burning particles by single particle aerosol mass spectrometer in the urban area of PRD, China, Atmos. Environ., 45, 3447–3453, 2011. Bowers, K. N., Choularton, T. W., Gallagher, M. W., Beswick, K. M., Flynn, M. J., Allen, A. G., Davison, B. M., James, J. D., Robertson, J. L., Harrison, R. M., Hewitt, C. N., Cape, J. N., McFadyen, G. G., Milford, C., Sutton, M. A., Martinsson, B. G., Frank, G., Swietlicki, E., Zhou, J., Berg, O. H., Mentes, B., Papapiropoulos, G., Hansson, H.-C., Leck, C., Kulmala, M., Aalto, P., Vakeva, M., Berner, A., Bizjak, M., Fuzzi, S., Laj, P., Facchini, M.-C., Orsi, G., Ricci, L., Nielsen, M., Allan, B. J., Coe, H., McFiggans, G., Plane, J. M. C., Collett Jr., J. L., Moore, K. F., and Sherman, D. E.: ACE-2 HILLCLOUD, An overview of the ACE-2 ground-based cloud experiment, Tellus B, 52, 750–778, 2000. Brenguier, J.-L., Pawlowska, H., and Schuller, L.: Cloud microphysical and radiative properties for parameterization and satellite monitoring of the indirect effect of aerosol on climate, J. Geophys. Res., 108, 8632, http://dx.doi.org/10.1029/2002JD002682doi:10.1029/2002JD002682, 2003. Chand, D., Anderson, T. L., Wood, R., Charlson, R. J., Hu, Y., Liu, Z., and Vaughan, M.: Quantifying above-cloud aerosol using spaceborne lidar for improved understanding of cloudy-sky direct climate forcing, J. Geophys. Res.,113, D13206, doi:10:10.1029/2007JD009433, 2008. Chand, D., Hegg, D. A., Wood, R., Shaw, G. E., Wallace, D., and Covert, D. S.: Source attribution of climatically important aerosol properties measured at Paposo (Chile) during VOCALS, Atmos. Chem. Phys., 10, 10789–10801, http://dx.doi.org/10.5194/acp-10-10789-2010doi:10.5194/acp-10-10789-2010, 2010. Chuang, P. Y., Collins, D. R., Pawlowska, H., Snider, J. R., Jonsson, H. H., Brenguier, J.-L., Flagan, R. C., and Seinfeld, J. H.: CCN measurements during ACE-2 and their relationship to cloud microphysical properties, Tellus, 52B, 843–867, 2000. Durkee, P. A., Noone, K. J., Ferek, R. J., Johnson, D. W., Taylor, J. P., Garrett, T. J., Hobbs, P. V., Hudson, J. G., Bretherton, C. S., Innis, G., Frick, G. M., Hoppel, W. A., O'Dowd, C. D., Russell, L. M., Gasparovic, R., Nielsen, K. E., Tessmer, S. A., Ostrom, E., Osborne, S. R., Flagan, R. C., Seinfeld, J. H., and Rand, H.: The Impact of Ship-Produced Aerosols on the Microstructure and Albedo of Warm Marine Stratocumulus Clouds, A Test of the MAST Hypothesis Li and Lii, J. Atmos. Sci., 57, 2554–2569, 2000. Dusek, U., Frank, G. P., Hildebrandt, L., Curtius, J., Schneider, J., Walter, S., Chand, D., Drewnick, F., Hings, S., Jung, D., Borrmann, S., and Andreae, M. O.: Size matters more than chemistry for cloud-nucleating ability of aerosol particles, Science, 312, 1375–1378, 2006. Dusek, U., Frank, G. P., Curtius, J., Drewnick, F., Schneider, J., Kurten, A., Rose, D., Andreae, M. O., Borrmann, S., and Pöschl, U.: Enhanced organic mass fraction and decreased hygroscopicity of cloud condensation nuclei (CCN) during new particle formation events, Geophys. Res. Lett., 37, L03804, http://dx.doi.org/10.1029/2009GL040930doi:10.1029/2009GL040930, 2010. Furutani, H., Dall'osto, M., Roberts, G., and Prather, K. A.: Assessment of the relative importance of atmospheric aging on CCN activity derived from field measurements, Atmos. Environ. , 42, 3130–3142, 2008. Gasso, S. and Hegg, D. A.: On the retrieval of columnar aerosol mass and CCN concentration by MODIS, J. Geophys. Res., 108, 4010, http://dx.doi.org/10.1029/2002JD002382doi:10.1029/2002JD002382, 2003. Guazzotti, S. A., Coffee, K. R., and Prather, K. A.: Continuous measurements of size-resolved particle chemistry during INDOX-Intensive Field Phase 99, J. Geophys. Res., 106, 28607–28627, 2001. Hawkins, L. N., Russell, L. M., Covert, D. S., Quinn, P. K., and Bates, T. S.: Carboxylic acids, sulfates, and organosulfates in processed continental organic aerosol over the southeast Pacific Ocean during VOCALS-Rex 2008, J. Geophys. Res., 115, D13201, http://dx.doi.org/10.1029/2009JD013276doi:10.1029/2009JD013276, 2010. Haywood, J. M., Osborne, S. R., Francis, P. N., Keil, A., Formenti, P., Andreae, M. O., and Kaye, P. H.: The mean physical and optical properties of regional haze dominated by biomass burning aerosol measured from the C-130 aircraft during SAFARI 2000, J. Geophys. Res., 108, D138473, http://dx.doi.org/10.1029/2002JD002226doi:10.1029/2002JD002226, 2003. Hegg, D. A., Nielsen, K., Covert, D. S., Jonsson, H. H., and Durkee, P. A.: Factors influencing the mesoscale variations in marine stratocumulus albedo, Tellus B, 59, 66–76, 2007. Hegg, D. A., Covert, D. S., and Jonsson, H. H.: Measurements of size-resolved hygroscopicity in the California coastal zone, Atmos. Chem. Phys., 8, 7193–7203, http://dx.doi.org/10.5194/acp-8-7193-2008doi:10.5194/acp-8-7193-2008, 2008. Hegg, D. A., Covert, D. S., Jonsson, H. H., and Woods, R.: Differentiating natural and anthropogenic cloud condensation nuclei in the California coastal zone, Tellus B, 61, 669–676, 2009. Hegg, D. A., Covert, D. S., Jonsson, H. H., and Woods, R. K.: The contribution of anthropogenic aerosols to aerosol light-scattering and CCN activity in the California coastal zone, Atmos. Chem. Phys., 10, 7341–7351, http://dx.doi.org/10.5194/acp-10-7341-2010doi:10.5194/acp-10-7341-2010, 2010. Henning, S., Wex, H., Henning, T., Kislev, A., Snider, J. R., Rose, D., Dusek, U., Frank, G. P., Poschl, U., Kristensson, A., Bilde, M., Tillman, R., Kiendler-Schnarr, A., Mentel, T. F., Walter, S., Schneider, J., Wennrich, C., and Stratmann, F.: Soluble mass, hygroscopic growth, and droplet activation of coated soot particles during LACIS Experiment in November (LexNo), J. Geophys. Res., 115, D11206, http://dx.doi.org/10.1029/2009JD012626doi:10.1029/2009JD012626, 2010. Hudson, J. G.: Effects of CCN concentration on stratus clouds, J. Atmos. Sci., 40, 480–486, 1983. Hoppel, W., Fitzgerald, J., Frick, G., Larson, R., and Mack, E: Aerosol size distributions and optical properties found in the marine boundary layer over the Atlantic Ocean, J. Geophys. Res., 95, 3659–3686, http://dx.doi.org/10.1029/JD095iD04p03659doi:10.1029/JD095iD04p03659, 1990. Hudson, J. G.: Variability of the relationship between particle size and cloud-nucleating ability, Geophy. Res. Lett., 34, L08801, http://dx.doi.org/10.1029/2006GL028850doi:10.1029/2006GL028850, 2007. Hudson, J. G. and Noble, S.: CCN and cloud droplet concentrations at a remote ocean site, Geophys. Res. Lett., 36, L13812, http://dx.doi.org/10.1029/2009GL038465doi:10.1029/2009GL038465, 2009. Hudson, J. G., Noble, S., and Jha, V.: Stratus cloud supersaturations, Geophys. Res. Lett., 37, L21813, http://dx.doi.org/10.1029/2010GL045197doi:10.1029/2010GL045197, 2010. Huneeus, N., Gallardo, L., and Rutllant, J. A.: Offshore transport episodes of anthropogenic sulfur in Northern Chile: potential impact on the stratocumulus cloud deck, Geophys. Res. Lett., 33, L19819, http://dx.doi.org/10.1029/2006GL026921doi:10.1029/2006GL026921, 2006. IPCC, Climate Change: The Scientific Basis: contributions of Working Group I to the Third Assessment Report of the IPCC, edited by: Houghton, J. T., Ding, Y., Griggs, D. J., Noguer, M., van der Linden, P. J., Dai, X., Maskell, K., and Johnson, C. A., Cambridge University Press, New York, 881 pp., 2001. IPCC, Climate Change: The Physical Science Basis: contribution of Working Group 1 to the Fourth Assessment Report of the IPCC, edited by: Solomon, S., Qin, D., Manning, M., Chen, Z., Marquis, M., Averyt, K. B., Tignor, M., and Miller, H. L., Cambridge University Press, New York, 996 pp., 2007 Jurányi, Z., Gysel, M., Weingartner, E., DeCarlo, P. F., Kammermann, L., and Baltensperger, U.: Measured and modelled cloud condensation nuclei number concentration at the high alpine site Jungfraujoch, Atmos. Chem. Phys., 10, 7891–7906, http://dx.doi.org/10.5194/acp-10-7891-2010doi:10.5194/acp-10-7891-2010, 2010. Kaku, K. C., Hegg, D. A., Covert, D. S., Santarpia, J. L., Jonsson, H., Buzorius, G., and Collins, D. R.: Organics in the Northeastern Pacific and their impacts on aerosol hygroscopicity in the subsaturated and supersaturated regimes, Atmos. Chem. Phys., 6, 4101–4115, http://dx.doi.org/10.5194/acp-6-4101-2006doi:10.5194/acp-6-4101-2006, 2006. Kapustin, V. N., Clarke, A. D., Shinozuka, Y., Howell, S., Brekhovskikh, Nakajima, T., and Higurashi, A.: On the determination of cloud condensation nuclei from satellites: challenges and possibilities, J. Geophys. Res., 111, D04202, http://dx.doi.org/10.1029/2004JD005527doi:10.1029/2004JD005527, 2006. Keil, A. and Haywood, J. M.: Solar radiative forcing by biomass burning aerosol particles during SAFARI 2000: a case study based on measured aerosol and cloud properties, J. Geophys. Res., 108, 8467, http://dx.doi.org/10.1029/2002JD002315doi:10.1029/2002JD002315, 2003. Klein, S. A. and Hartmann, D. L.: The seasonal cycle of low stratiform clouds, J. Climate, 6, 1587–1606, 1993. Kleinman, L. I., Daum, P. H., Lee, Y.-N., Lewis, E. R., Sedlacek III, A. J., Senum, G. I., Springston, S. R., Wang, J., Hubbe, J., Jayne, J., Min, Q., Yum, S. S., and Allen, G.: Aerosol concentration and size distribution measured below, in, and above cloud from the DOE G-1 during VOCALS-REx, Atmos. Chem. Phys., 12, 207–223, http://dx.doi.org/10.5194/acp-12-207-2012doi:10.5194/acp-12-207-2012, 2012. Kogan, Z. N., Kogan, Y. L., and Lilly, D. K.: Evaluation of sulfate aerosols indirect effect in marine stratocumulus clouds using observation-derived cloud climatology, Geophys. Res. Lett., 23, 1937–1940, 1996. Leaitch, W. R., Banic, C. M., Isaac, G. A., Couture, M. D., Liu, P. S. K., Gultepe, I., and Li, S.-M.: Physical and chemical observations in marine stratus during the 1993 North Atlantic Regional Experiment: Factors controlling cloud drop number concentrations, J. Geophys. Res., 101, 29123–29135, 1996. Li, W. J. and Shao, L. Y.: Mixing and water-soluble characteristics of particulate organic compounds in individual urban aerosol particles, J. Geophys. Res., 115, D02301, http://dx.doi.org/10.1029/2009JD012575doi:10.1029/2009JD012575, 2010. Lu, M.-L., Conant, W. C., Jonsson, H. H., Varutbangkul, V., Flagan, R. C., and Seinfeld, J. H.: The Marine Stratus/Stratocumulus Experiment (MASE): Aerosol-cloud relationships in marine stratocumulus, J. Geophys. Res., 112, D10209, http://dx.doi.org/10.1029/2006JD007985doi:10.1029/2006JD007985, 2007. Lu, M.-L., Feingold, G., Jonsson, H. H., Chuang, P. Y., Gates, H., Flagan, R. C., and Seinfeld, J. H.: Aerosol-cloud relationship in continental shallow cumulus, J. Geophys. Res., 113, D15201, http://dx.doi.org/10.1029/2007JD009254doi:10.1029/2007JD009254, 2008. Martin, G. M., Johnson, D. W., and Spice, A.: The measurement and parameterization of effective radius of droplets in warm stratocumulus clouds, J. Atmos. Sci., 51, 1823–1842, 1994. McFiggans, G., Artaxo, P., Baltensperger, U., Coe, H., Facchini, M. C., Feingold, G., Fuzzi, S., Gysel, M., Laaksonen, A., Lohmann, U., Mentel, T. F., Murphy, D. M., O'Dowd, C. D., Snider, J. R., and Weingartner, E.: The effect of physical and chemical aerosol properties on warm cloud droplet activation, Atmos. Chem. Phys., 6, 2593–2649, http://dx.doi.org/10.5194/acp-6-2593-2006doi:10.5194/acp-6-2593-2006, 2006. Middlebrook, A. M., Murphy, D. M., and Thomson, D. S.: Observations of organic material in individual marine particles at Cape Grim during the First Aerosol Characterization Experiment (ACE-1), J. Geophys. Res., 103, 16475–16483, 1998. Neususs, C., Pelzing, M., Plewka, A., and Herrmann, H.: A new analytical approach for size-resolved speciation of organic compounds in atmospheric aerosol particles: Methods and first results, J. Geophys. Res., 105, 4513–4527, http://dx.doi.org/10.1029/1999JD901038doi:10.1029/1999JD901038, 2000. Oppo, C., Bellandi, S., Innocenti, N. D., Stortini, A. M., Loglio, G., Schiavuta, E., and Cini, R.: Surfactant components of marine organic matter as agents for biogeochemical fractionation and pollutant transport via marine aerosols, Mar. Chem., 63, 235–253, 1999. Petters, M. D. and Kreidenweis, S. M.: A single parameter representation of hygroscopic growth and cloud condensation nucleus activity, Atmos. Chem. Phys., 7, 1961–1971, http://dx.doi.org/10.5194/acp-7-1961-2007doi:10.5194/acp-7-1961-2007, 2007. Petters, M. D. and Kreidenweis, S. M.: A single parameter representation of hygroscopic growth and cloud condensation nucleus activity – Part 2: Including solubility, Atmos. Chem. Phys., 8, 6273–6279, http://dx.doi.org/10.5194/acp-8-6273-2008doi:10.5194/acp-8-6273-2008, 2008. Platnick, S. and Twomey, S.: Determining the susceptibility of cloud albedo to changes in droplet concentration with the Advanced Very High Resolution Radiometer, J. Appl. Meteor., 33, 334–347, 1994 Pratt, K. A. and Prather, K. A.: Aircraft measurements of vertical profiles of aerosol mixing states, J. Geophys. Res., 115, D11305, http://dx.doi.org/10.1029/2009JD013150doi:10.1029/2009JD013150, 2010. Pringle, K. J., Carslaw, K. S., Spracklen, D. V., Mann, G. M., and Chipperfield, M. P.: The relationship between aerosol and cloud drop number concentrations in a global aerosol microphysics model, Atmos. Chem. Phys., 9, 4131–4144, http://dx.doi.org/10.5194/acp-9-4131-2009doi:10.5194/acp-9-4131-2009, 2009. Remer, L. A., Kaufman, Y. J., Tanre, D., Mattoo, S., Chu, D. A., Martins, J. V., Li, R.-R., Ichoku, C., Levy, R. C., Kleidman, R. G., Eck, T. F., Vermote, E., and Holben, B. N.: The MODIS aerosol algorithm, products, and validation, J. Atmos. Sci., 62, 947–973, 2005. Roberts, G., Mauger, G., Hadley, O., and Ramanathan, V.: North American and Asian aerosols over the eastern Pacific Ocean and their role in regulating cloud condensation nuclei, J. Geophys. Res., 111, D13205, http://dx.doi.org/10.1029/2005JD006661doi:10.1029/2005JD006661, 2006. Stevens, B. and Feingold, G.: Untangling aerosol effects on clouds and precipitation in a buffered system, Nature, 461, 607–613, 2009. Swietlicki, E., Zhou, J., Covert, D. S., Hameri, K., Busch, B., Vakeva, M., Dusek, U., Berg, O. H., Widensohler, A., Aalto, P., Makela, P., Martinsson, B. G., Papaspiropoulos, G., Mentes, B., Frank, G., and Stratmann, F.: Hygroscopic properties of aerosol particles in the northeastern Atlantic during ACE-2, Tellus B, 52, 201–227, 2000. Twohy, C. H., Petters, M. D., Snider, J. R., Stevens, B., Tahnk, W., Wetzel, M., Russell, L., and Burnet, F.: Evaluation of the aerosol indirect effect in marine stratocumulus clouds: droplet number, size, liquid water path, and direct radiative impact, J. Geophys. Res., 110, D08203, http://dx.doi.org/10.1029/2004JD005116doi:10.1029/2004JD005116, 2005. Twomey, S.: The nuclei of natural cloud formation, II: The supersaturation in natural clouds and the variation of cloud droplet concentration, Pure Appl. Geophys., 43, 243–249, 1959. Wang, J., Flagan, R. C., Seinfeld, J. H., Jonsson, H. H., Collins, D. R., Russell, P. B., Schmid, B., Redemann, J., Livingston, J. M., Gao, S., Hegg, D. A., Welton, E. J., and Bates, D.: Clear-column radiative closure during ACE-Asia: Comparison of multiwavelength extinction derived from particle size and composition with results from Sun photometry, J. Geophys. Res., 107, 4688, http://dx.doi.org/10.1029/2002JD002465doi:10.1029/2002JD002465, 2002. Wang, J., Daum, P. H., Kleinman, L. I., Lee, Y. N., Schwartz, S. E., Springston, S. R., Jonsson, H., Covert, D., and Elleman, R.: Observation of ambient aerosol particle growth due to in-cloud processes within boundary layers, J. Geophys. Res., 112, D14207, http://dx.doi.org/10.1029/2006JD007989doi:10.1029/2006JD007989, 2007. Warren, S. G., Hahn, C. J., London, J., Chervin, R. M., and Jenne, R. L. : Global Distribution of Total Cloud Cover and Cloud type Amounts Over the Ocean, NCAR Technical Note NCAR/TN-317+STR, 1988.